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Title: Short-Range Disorder in TeO2 Melt and Glass

Abstract

High-resolution X-ray pair distribution functions for molten and glassy TeO2 reveal coordination numbers nTeO ≈ 4. However, distinct from the known α-, β-, and γ-TeO2 polymorphs, there is considerable short-range disorder such that no clear cutoff distance between bonded and nonbonded interactions exists. We suggest that this is similar to disorder in δ-TeO2 and arises from a broad distribution of asymmetric Te–O–Te bridges, something that we observe becomes increasingly asymmetric with increasing liquid temperature. Such behavior is qualitatively consistent with existing interpretations of Raman scattering spectra, and equivalent to temperature-induced coordination number reduction, for sufficiently large cutoff radii. Therefore, TeO2 contains a distribution of local environments that are, furthermore, temperature dependent, making it distinct from the canonical single-oxide glass formers. Furthermore, our results are in good agreement with high-level ab initio cluster calculations.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [4]; ORCiD logo [5];  [3];  [3];  [3];  [6]
  1. Materials Development, Inc., Arlington Heights, IL (United States); Rutherford Appleton Lab., Oxon (United Kingdom)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Coe College, Cedar Rapids, IA (United States)
  4. National Hellenic Research Foundation, Athens (Greece)
  5. Max-Planck-Inst. für Kohlenforschung, Mülheim an der Ruhr (Germany)
  6. Materials Development, Inc., Arlington Heights, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)
OSTI Identifier:
1591765
Grant/Contract Number:  
AC02-06CH11357; SC0018601; NSF-DMR 1746230; NSRF 2014-2020; MIS 5002409
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 11; Journal Issue: 2; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; glass; melt

Citation Formats

Alderman, O. L. G., Benmore, C. J., Feller, S., Kamitsos, E. I., Simandiras, E. D., Liakos, D. G., Jesuit, M., Boyd, M., Packard, M., and Weber, R. Short-Range Disorder in TeO2 Melt and Glass. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.jpclett.9b03231.
Alderman, O. L. G., Benmore, C. J., Feller, S., Kamitsos, E. I., Simandiras, E. D., Liakos, D. G., Jesuit, M., Boyd, M., Packard, M., & Weber, R. Short-Range Disorder in TeO2 Melt and Glass. United States. https://doi.org/10.1021/acs.jpclett.9b03231
Alderman, O. L. G., Benmore, C. J., Feller, S., Kamitsos, E. I., Simandiras, E. D., Liakos, D. G., Jesuit, M., Boyd, M., Packard, M., and Weber, R. Mon . "Short-Range Disorder in TeO2 Melt and Glass". United States. https://doi.org/10.1021/acs.jpclett.9b03231. https://www.osti.gov/servlets/purl/1591765.
@article{osti_1591765,
title = {Short-Range Disorder in TeO2 Melt and Glass},
author = {Alderman, O. L. G. and Benmore, C. J. and Feller, S. and Kamitsos, E. I. and Simandiras, E. D. and Liakos, D. G. and Jesuit, M. and Boyd, M. and Packard, M. and Weber, R.},
abstractNote = {High-resolution X-ray pair distribution functions for molten and glassy TeO2 reveal coordination numbers nTeO ≈ 4. However, distinct from the known α-, β-, and γ-TeO2 polymorphs, there is considerable short-range disorder such that no clear cutoff distance between bonded and nonbonded interactions exists. We suggest that this is similar to disorder in δ-TeO2 and arises from a broad distribution of asymmetric Te–O–Te bridges, something that we observe becomes increasingly asymmetric with increasing liquid temperature. Such behavior is qualitatively consistent with existing interpretations of Raman scattering spectra, and equivalent to temperature-induced coordination number reduction, for sufficiently large cutoff radii. Therefore, TeO2 contains a distribution of local environments that are, furthermore, temperature dependent, making it distinct from the canonical single-oxide glass formers. Furthermore, our results are in good agreement with high-level ab initio cluster calculations.},
doi = {10.1021/acs.jpclett.9b03231},
journal = {Journal of Physical Chemistry Letters},
number = 2,
volume = 11,
place = {United States},
year = {2019},
month = {12}
}

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